Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Pei Nian,Xiaojuan Wang,Shuming Li,Zheng Wang,Yibin Wei
There remains a great challenge to develop a switchable and feasible membrane for integrate reversible separation of oil/water mixtures. Herein, a highly-quality CAU-10-H mesh membrane with switchable superwettability was fabricated via solvothermal synthesis for on-demand oil/water separation. The CAU-10-H membrane exhibited under-liquid dual superlyophobicity due to the hierarchical micro-/nanostructures constructed by interpenetrating CAU-10-H crystals grown on the mesh. Meanwhile, the secondary growth time affecting the wetting behavior of the membrane is studied. More importantly, the membrane can achieve both immiscible oil/water separation and emulsion separation with high separation flux and high efficiency (>99.9%). Moreover, the membrane shows an excellent anti-corrosive property in various harsh environment. The present development would provide novel insights into the rational fabrication of MOF-based membranes for on-demand oil/water separation.
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JOURNAL OF CATALYSIS
·
2023
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IF 7.3
Jin Yuan,Zhiwei He,Hongbo Zhang
Selective C–H bond oxidation of cyclohexane into KA oil (ketone-alcohol) is of vital importance in both fundamental research and industrial applications while limited by complex reaction network and suffering from low efficiency. In this study, Ce(OH)SO 4 · x H 2 O was chosen as a probe to systematically investigate the C–H bond activation and C–C bond rupture as a function of various reaction parameters, including the reactant/product concentrations, catalyst applied, reaction temperatures, acidic concentrations etc, and found that bi-molecule of C 6 H 12 was probably involved in both C–H bond rupture and C–C bond cleavage and both were controlled by one deprotonation elementary step with ·O 2 – and h + as the key active components, which were supported by parity fittings and primary KIEs determined. In addition, the C–C bond rupture was found to be mainly following C 6 H 10 O to ε-caprolactone and further to linear acids reaction path. Hopefully, this study could help people find/optimize reaction systems in selective hydrocarbon upgradings.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2023
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IF 5.7
Mao Chen,Bingbing Fan,Haoyuan Lei,Zijie Song,Shaojun Zhang,Hailong Wang,Rui Zhang,Hongxia Li,Yongqiang Chen
Large size high density h-BN/ZrO 2 composites (ø = 110 mm, h = 15 mm) were rapidly prepared by spark plasma sintering (SPS) with sintering cycle 20 min. The effects of additives on the mechanical properties , microstructure evolution, and corrosion resistance of the h-BN/ZrO 2 composites were studied. The Al 2 O 3 , MgO , SiO 2 , La 2 O 3 and ZrO 2 rapidly formed heterogeneous eutectic crystals under the action of SPS. The low eutectic compounds significantly promoted the diffusion of h-BN or ZrO 2 , also increased the density. The flexural strength of h-BN/ZrO 2 composites could reach 196.31 MPa, and the apparent porosity was only 0.42 %. The additives are combined with zirconia to form a high viscosity eutectic, whose corrosion resistance to molten steel is obviously better than that of single ZrO 2 . The corrosion depth of h-BN/ZrO 2 composites was only 114 µm after corroded in molten steel at 1550 °C for 80 min. The comprehensive properties of h-BN/ZrO 2 composites were obviously improved by appropriate additives.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Wei Li,Ting Luo,Changxu Zhu,Bin Zhang,Bingqiang Cao
Graphene/hexagonal boron nitride nanocomposites with different dimensions have great application prospects in the field of lubrication due to their unique layered structure and excellent mechanical properties. However, due to their complex synthesis process, easy agglomeration, and poor stability, graphene/hexagonal boron nitride nanocomposites have not yet been applied in lubricating applications. Herein, a simple and green in situ laser irradiation method is proposed to construct two-dimensional (2D) reduced graphene oxide (rGO) nanosheets and zero-dimensional (0D) hexagonal boron nitride nanosphere 2D/0D nanocomposite (L-rGO/h-BN). During the one-step laser irradiation in liquid, the GO nanosheets were reduced to rGO nanosheets. Meanwhile, the hexagonal boron nitride (h-BN) transformed from nanoflakes to nanospheres via a pulsed laser heating and reshaping process and embedded into the multilayer graphene nanosheets. The spherical h-BN nanoparticles as interlayer support can maintain the 2D graphene with a more stable layered structure, while the insertion of graphene sheets also effectively inhibits the agglomeration of the spherical h-BN nanoparticles. Therefore, a hierarchical 2D/0D layered rGO/h-BN nanocomposite was formed. Importantly, such composite nanoparticles can well disperse in the lubricating oil without significant precipitation for over 30 days and show remarkably improved tribological performance. This is due to the synergistic lubricant effect of the deposition repair effect from rGO nanosheets reducing wear and micro-bearing effect from h-BN nanospheres reducing friction by changing sliding friction into rolling friction.
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ELECTROCHIMICA ACTA
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2022
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IF 7.336
Geng Cheng,Zhen Li,Erli Qu,Shan Ren,Dongmei Han,Min Xiao,Shuanjin Wang,Yuezhong Meng
It's of significant importance for the development of proton exchange membranes with low phosphoric acid (PA) uptake, high proton conductivity, better proton conduction stability and low production-costs for high temperature proton exchange membrane fuel cells (HT-PEMFCs). Featured with variable structure and diversified functionality, porous organic networks are newly emerged filler materials for polyelectrolytes in energy conversion field. In this work, a typical Schiff-base type porous polymeric network (SNW-1) with abundant N H sites was synthesized and blended with ether-type polybenzimidazole (PBI) for the first time. The thermal and chemical stability of the as-prepared composite membranes completely satisfy the practical requirements of HT-PEMFCs. The constructed consecutive proton conduction channels endow the composite membranes higher proton conductivity with low PA uptake. When the doping content of SNW-1 reached 30%, the PBI/30%-SNW-1 membrane showed much higher proton conductivity with lower PA uptake (114.0 mS cm −1 , 175.0%) comparing with those of the pristine PBI (67.3 mS cm −1 , 270.0%) at 160 °C. The PBI/ x %-SNW-1 membranes also exhibited better proton conduction stability. After 30 h of long-time evaluation at 140 °C, PBI/30%-SNW-1 composite membrane gives only an 8.47% decay of proton conductivity, which is lower than that of the pristine PBI (12.84%). The preparation procedure of PBI/ x %-SNW-1 composite membranes is simple, which provides a potential pathway for the development of high-performance proton exchange membrane for HT-PEMFCs.
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FUEL
·
2022
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IF 8.035
Mengjiao Xing,Yunlei Chen,Jian Cao,Yuanlong Han,Zhichao Tao,Fei Wang,Kun Hao,Ling Zhang,Wentao Zheng,Hongwei Xiang,Yong Yang,Yongwang Li,Xiaodong Wen
Understanding the catalytic structure–activity relationship over active sites is of fundamental importance in heterogeneous catalysis field. Herein, a series of H-ZSM-5 zeolites with Al pairs contents in the range of 31% to 82% are used to explore the structure sensitivity of olefin aromatization reaction. Compared with high reaction temperatures (385 ℃ and above), prominently different initial aromatic yields are observed over the samples at 150 ℃. In addition, the 1-octene temperature-programmed surface reaction (TPSR) and theoretical calculation results give a thorough understanding on active site dependent activation temperature (100 vs 150 ℃ over Al pairs and single Al). However, the catalytic cycle of olefin aromatization is not sustainable at low reaction temperature, which is due to the formation and blocking of big molecules in the micropores (e.g., trimethylbenzene etc.). In conclusion, the desorption of big molecules is the rate-determining step for olefin aromatization reaction over H-ZSM-5, which masks the structure sensitivity over Al pairs and single Al.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Zhihui Wei,Jie Li,Lixia Yang,Siyu Liu,Haicheng Li,Mingxia Lu,Tiantian Ying,Yan Luo,Kexin Li,Zhenglin Chen,Xiuping Zhang,Shenglian Luo
Degradation of halogenated organic compounds using the electro-reduction process is a promising approach for advanced water treatment. In this work, antiferromagnetic Co 3 O 4 nanoparticles were first loaded on a uniform anodic porous TiO 2 surface through a hydrothermal strategy, then subjected to an electrochemical reduction, which transform from nanoparticle-shape to interconnected nanoflakes. Compared with the pristine Co 3 O 4 nanoparticles, the morphologically transformed Co 3 O 4 cathode features a porous interface with amorphous Co(OH) 2 and CoOOH shell, which favors the generation of abundant •OH radicals along with lower overpotential for reducing H + to H*. On account of the plentiful radicals and self-supporting nature, the resulting Co 3 O 4 cathode retains high activity for efficiently degrading Thiamphenicol in water, even after 10 h run, demonstrating remarkable durability. Moreover, it is adaptable in a wide pH window of 3 to 10, and effectual when the initial Thiamphenicol concentration increases from 0.5 to 50 mg/L regardless of the water background (tap water, lake water, or river water). This study delivers a profound cognition about the dynamic behaviors of Co 3 O 4 -based electrocatalysts applied in eliminating halogenated antibiotics.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Yong Zeng,Yizhen Chen,Di Sha,Yuchao Wu,Renhui Qiu,Wendi Liu
Thermoplastic polyurethane (TPU) elastomers are widely used in daily products owing to their flexible structures and decent mechanical properties. Vegetable oils (VOs) are promising renewable resources for polymer synthesis with readily availability and abundant derivatives. However, most VO-based polyurethanes are usually thermosets with an unsatisfactory material performance because the C═C bonds are randomly located on triglyceride long chains. Herein, a biobased TPU elastomer was facilely synthesized from palm oil (PO) with desirable and tunable mechanical properties. PO-based diol was synthesized from PO via amidation with 2-(2-hydroxyethylamino)ethanol. The resulting PO diethanolamide (POEA), combined with biobased butane-1,4-diol, was further reacted with 1,6-diisocyanatohexane to prepare PO-based TPU elastomers. The elastomers containing abundant H-bonds from carbamates in the backbone and dangling fatty acid side chains exhibited a microphase separation structure, endowing the elastomers with superior stretchability (up to a strain of 831%), restorability, and self-healing ability. The morphological, melting, crystallization, and rheological behaviors of the elastomers were fully studied. The dynamic and reversible three-dimensional cross-linked network consisting of van der Waals forces and H-bonds was investigated to reveal the formation mechanism of the elastomers.
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ENVIRONMENTAL RESEARCH
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2022
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IF 8.431
Xiang Meng,Jianlong Wang,Lejin Xu
To further improve the treatment capacity of actual wastes, H + was introduced into the homogeneous Fenton system as a co-catalyst for dissolution and degradation of the mixed nuclear-grade cationic and anionic exchange resins. The effects of acid type and concentration, catalyst type and concentration, H 2 O 2 dosage, initial temperature, antifoaming agent and resin ratio were studied. The concentration of inorganic acid , type and concentration of catalyst had significant influence on the decomposition of mixed resins. The experimental results showed that when the mixing ratio of resins was 1:1, the initial temperature was 96 ± 1 °C, the amount of H 2 O 2 was 200 mL, and the concentration of H + /Fe 2+ was 1 M/0.1 M, complete dissolution and 79% weight reduction of mixed resins were obtained. Combined with density functional theory (DFT) calculations, cationic exchange resin and anionic exchange resin showed different reactivity in the experiment. Hydroxyl radicals (•OH) tended to attack –SO 3 - groups with more negative charges, and the barrier energy of –SO 3 - ion dissociation was 8.2 kcal/mol, which caused the cationic exchange resin to be easily destroyed. According to the characterization results, the characteristic intermediates were determined, indicating that desulfonation, valence change of nitrogen atom , and cleavage of long-chain carbon skeleton existed during the reaction, but incomplete oxidation still remained.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Dongxue Zhou,Xiangdong Xue,Xing Wang,Qingjie Luan,Ang Li,Liguo Zhang,Baozhen Li,Wenjun Dong,Ge Wang,Changmin Hou
Element doping is an excellent strategy to promote charge separation and reaction kinetics of photocatalyst, which plays significant role in accelerating the sustainable energy development process. Herein, Ni, In co-doped ZnIn 2 S 4 photocatalyst was prepared by a microwave-assisted solvothermal method. The rapid crystallization of ZnIn 2 S 4 resulted in partial In atoms substituted Zn atom during the formation of [ZnS] 4 layer. In doping in tetrahedral Zn sites increases the electron delocalization around In sites, hence reduces the electronic potential wells along Z axis. Ni doping in tetrahedral Zn sites decreases the negative charge on the S sits, which balances the H adsorption/desorption, further boosting the photocatalytic activity. As a result, Ni, In co-doped ZnIn 2 S 4 possess an optimal photocatalytic H 2 evolution property of 21.94 μmol·h −1 , which is nearly 1.8 and 6.1 times of In-ZnIn 2 S 4 (11.78 μmol·h −1 ) and ZnIn 2 S 4 (3.6 μmol·h −1 ).
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Heng Ye,Shengnan Wang,Yong Wang,Peiting Guo,Liying Wang,Chengke Zhao,Shuqing Chen,Yimai Chen,Hongqi Sun,Shaobin Wang,Xing Ma
Wastewater remediation using micro/nanomotors is a hot topic, and MnO 2 based materials have become fascinating alternatives to rare noble metal-based micro/nanomotors. Herein, we demonstrate facile and large-scale synthesis of Fe-MnO 2 core-shell micromotors for antibiotic pollutant removal. Heat-treatment results in a phase transformation of MnO 2 with formation of iron oxides and partially exfoliates the MnO 2 nanoplate shell structure to promote mobility. The iron-manganese oxide micromotors exhibit an efficient removal of tetracycline antibiotics via a combination of catalytic degradation and adsorptive bubble separation. For the first time, atomic H* was found to participate in the micromotor-assisted degradation process, resulting in optimal Fenton reaction in neutral conditions with a good decontamination performance. Owing to the merits of abundance, magnetic recovery, facile fabrication, good motion, and environmental friendliness, as well as decontamination performance in a wide pH range, these core-shell micromotors demonstrate a promising candidate in practical wastewater treatment .
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 6
·1788-1798
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IF 6.177
Jing Zhao,Yanzhuo Zhang,Hucheng Zhang,Haiyan Wang,Jianji Wang
Hydrogen spillover is an important theme for hydrogen storage and H-involving catalytic reactions. This work shows that catalytic reactivity and selectivity can be revealed by differentiating the energetic characteristics of spilled H species. With the assistance of Ti, F and C in MXenes, Pd1.8Ni@Ti3C2Tx presents a high capacity for spillover hydrogen storage at ambient temperatures, and the rich oxygenated groups act as the main carriers of hydrogen spillover around metal nanoparticles. Thermodynamic analysis reveals that the catalytic performances are energetically dominated by the adsorption enthalpies of the active spilled H species rather than the amount of spillover hydrogen, and can be tuned by alloying and surface modification. The ideas are verified from the excellent catalysis, chemoselectivity and stereoselectivity of Pd1.8Ni@Ti3C2Tx in semihydrogenations. The strategy of maximizing catalytic performances is applicable to other Pd-based bimetals@Ti3C2Tx, such as Pd2.6Co@Ti3C2Tx and Pd1.5Fe@Ti3C2Tx, and provides new energetics perspectives to understand the catalytic mechanism in spillover-involving chemical procedures.
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